Mode-Specific Dynamics of Ammonia Dissociative Chemisorption on Ru(0001)

TL;DR

This study investigates how different vibrational modes of ammonia influence its dissociation on Ru(0001) surface, using advanced simulations on a newly developed potential energy surface to reveal mode-specific dynamics.

Contribution

The paper introduces a new 12-dimensional global potential energy surface for ammonia on Ru(0001), enabling detailed quasi-classical trajectory simulations of dissociation dynamics.

Findings

Strong mode specificity observed in ammonia dissociation.

Simulation results agree well with experimental data.

The PES facilitates future quantum dynamical studies.

Abstract

The mode specific dissociative chemisorption dynamics of ammonia on the Ru(0001) surface is investigated using a quasi-classical trajectory (QCT) method on a new global potential energy surface (PES) with twelve dimensions. The PES is constructed by fitting 92524 density functional theory points using the permutation invariant polynomial-neural network method, which rigorously enforces the permutation symmetry of the three hydrogen atoms as well as the surface periodicity. The PES enables highly efficient QCT simulations as well as future quantum dynamical studies of the scattering/dissociation dynamics. The QCT calculations yield satisfactory agreement with experiment and suggest strong mode specificity, in general agreement with the predictions of the Sudden Vector Projection model.